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dc.contributor.authorDavidson, Alisha L.
dc.contributor.authorWebb, Paul B.
dc.contributor.authorSilverwood, Ian P.
dc.contributor.authorLennon, David
dc.date.accessioned2020-04-21T15:30:03Z
dc.date.available2020-04-21T15:30:03Z
dc.date.issued2020-04-07
dc.identifier.citationDavidson , A L , Webb , P B , Silverwood , I P & Lennon , D 2020 , ' The application of quasi-elastic neutron scattering to investigate hydrogen diffusion in an iron-based Fischer-Tropsch synthesis catalyst ' , Topics in Catalysis , vol. First Online . https://doi.org/10.1007/s11244-020-01259-2en
dc.identifier.issn1022-5528
dc.identifier.otherPURE: 267545534
dc.identifier.otherPURE UUID: c6cf12d8-7be6-4953-b791-75a64dbec6d1
dc.identifier.otherWOS: 000524390000001
dc.identifier.otherORCID: /0000-0003-2532-344X/work/72842809
dc.identifier.otherScopus: 85083375788
dc.identifier.urihttp://hdl.handle.net/10023/19832
dc.descriptionSasol Ltd., (PGRS-3) the University of Glasgow and the Engineering and Physical Sciences Research Council (EP/P505534/1) are thanked for the provision of postgraduate studentship (ALD). The STFC Rutherford Appleton Laboratory is thanked for access to neutron beam facilities (RB1720188) [26]. The Royal Society are thanked for the provision of an Industrial Fellowship (PBW).en
dc.description.abstractIron-based Fischer–Tropsch synthesis (FTS) catalysts evolve in situ on exposure to synthesis gas (CO & H2) forming a mixture of iron oxides, iron carbides and carbonaceous deposits. Recently, the application of inelastic neutron scattering has shown the progressive formation of a hydrocarbonaceous overlayer during this catalyst conditioning period. The evolving nature of the catalyst alters the proportion of phases present within the catalyst, which may influence the transport of hydrogen within the reaction system. Preliminary quasi-elastic neutron scattering (QENS) measurements are used to investigate hydrogen diffusion within an un-promoted iron FTS catalyst that has experienced varying levels of time-on-stream (0, 12 and 24 h) of ambient pressure CO hydrogenation at 623 K. Measurements on the catalyst samples in the absence of hydrogen show the unreacted sample (t = 0 h) to exhibit little increase in motion over the temperature range studied, whereas the t = 12 and 24 h samples exhibit a pronounced change in motion with temperature. The contrast is attributed to the presence of the afore-mentioned hydrocarbonaceous overlayer. Measurements on the samples in the presence of liquid hydrogen show hydrogen diffusional characteristics to be modified as a function of the catalyst conditioning process but, due to the complexity of the evolving catalyst matrix, the hydrogen motion cannot be attributed to a particular phase or component of the catalyst. Problems in the use of hydrogen as a probe molecule in this instance are briefly considered. Coincident neutron diffraction studies undertaken alongside the QENS measurements confirm the transition from hematite pre-catalyst to that of Hägg carbide during the course of extended times-on-stream.
dc.format.extent8
dc.language.isoeng
dc.relation.ispartofTopics in Catalysisen
dc.rightsCopyright © The Author(s) 2020. Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.en
dc.subjectFischer-Tropsch synthesisen
dc.subjectQuasi-elastic neutron scatteringen
dc.subjectHydrogen diffusionen
dc.subjectQD Chemistryen
dc.subjectDASen
dc.subject.lccQDen
dc.titleThe application of quasi-elastic neutron scattering to investigate hydrogen diffusion in an iron-based Fischer-Tropsch synthesis catalysten
dc.typeJournal articleen
dc.description.versionPublisher PDFen
dc.contributor.institutionUniversity of St Andrews.School of Chemistryen
dc.identifier.doihttps://doi.org/10.1007/s11244-020-01259-2
dc.description.statusPeer revieweden


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